This study presents a novel solvent-free solid polymer electrolyte (SPE) with optimized phase tuning, enabling high ionic conductivity and high-resolution patterning via direct ink writing (DIW) simultaneously. The incorporation of a semi-interpenetrating polymer network (semi-IPN) structure enhances the mechanical properties, ensuring durability and flexibility. This advancement facilitates the development of arbitrarily shaped all-solid-state batteries (ASSBs) for wearable and flexible electronics.
Abstract
As demand for customized wearable electronics grows, free-form Li-ion batteries (LIBs) are attracting significant attention. Although substantial advancements have been made in printed LIBs for shape-versatile electronics, the development of printable solid-state electrolytes remains challenging due to the difficulty of simultaneously achieving desirable rheological properties and ionic conductivity. In this study, a solvent-free, non-flammable solid polymer electrolyte (SPE) is designed as a novel three-dimensional (3D) printable electrolyte via direct ink writing (DIW) for all-solid-state batteries (ASSBs). The solvent-free nature of this SPE eliminates post-annealing steps, enhancing safety by mitigating risks of leakage, short-circuiting, and fire. Additionally, precise control over polymer molecular weight and electrolyte composition enables high printing resolution (~100 μm), high ionic conductivity (0.705 mS cm−1 at 25°C), and intrinsic non-flammability. A 3D-printed ASSB, featuring a LiFePO4 cathode and Li4Ti5O12 anode with a mass loading of 7 mg cm−2, achieves a high areal capacity of 1.14 mAh cm−2, surpassing all previously reported directly printed ASSBs. This SPE facilitates scalable production of fully DIW-printed ASSBs with superior design flexibility and space efficiency, enabling printing onto customized targets such as flexible substrates and advancing the development of next-generation wearable electronics.
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